CN108290109A - Reduce the CO in industrial process2The method and system of discharge - Google Patents

Reduce the CO in industrial process2The method and system of discharge Download PDF

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Publication number
CN108290109A
CN108290109A CN201680066090.1A CN201680066090A CN108290109A CN 108290109 A CN108290109 A CN 108290109A CN 201680066090 A CN201680066090 A CN 201680066090A CN 108290109 A CN108290109 A CN 108290109A
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gas
fischer
gases
gas stream
tropsch
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T·达维迪安
S·哥图斯
C·比舒维尔
M·瑞坦比克
A·M·马雷克
P·E·赫鲁嫩代克
G·R·迈马
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Dow Global Technologies LLC
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Dow Global Technologies LLC
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    • B01D53/34—Chemical or biological purification of waste gases
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Abstract

It is a kind of to be used to reduce the CO in industrial process2The method and integrated system of discharge.The method and integrated system (100) capture carbon dioxide (CO using chemical absorbent from first gas stream (104)2) gas with generate compared with first gas stream with higher concentration carbon monoxide (CO) gas and low concentration CO2The second gas stream (106) of gas.CO gases in the second gas stream be used for hydrogen (H2) (138) exothermic reaction (108) in generate C5To C20Hydrocarbon.Using at least part of the heat generated in the exothermic reaction, by discharging the CO captured from the first gas stream2Gas (128) regenerates the chemical absorbent.The heat captured during the exothermic reaction can optionally be initially used for generating electricity, wherein remaining heat is for chemical absorbent described in hot recycling after power generation.

Description

Reduce the CO in industrial process2The method and system of discharge
Technical field
The present disclosure relates generally to industrial process, and more particularly relate to reduce the CO of the discharge gas from industrial process2 Gas discharges.
Background technology
Various industrial process, which generate, contains carbon dioxide (CO2) and other carbonaceous products (such as carbon monoxide (CO)) discharge Gas.The example of this kind of discharge gas includes from those of steel and iron manufacturing industry (such as blast furnace gas, oxygen converter gas or coke Producer gas).These discharge gases have the CO in about 10 to 50 percent by volume (volume %) ranges2Gas concentration and about 10 CO gas concentrations within the scope of to 80vol.%.Gas, which is discharged, can also contain other gases such as hydrogen, hydrocarbon and/or such as nitrogen Inert gas, amount can be of about 50 volume %.Flue gas is an example of discharge gas.
Before being discharged into the atmosphere, due to its toxicity, the CO gases in exhaust gas need to be converted into CO2Gas.It can make CO is generated with combustion process2Gas and the heat that can be used for various processes.However, high concentration CO2Gas and the significant reduction of nitrogen The calorie dense of CO gases present in gas is discharged, causes to decline using the enthusiasm of exhaust gas.Nevertheless, toxic/have Harmful CO gases must be converted to CO before discharge2Gas.Therefore, often discharge gas burns so that CO gases to be converted to separately Outer CO2Gas recycles the heat generated in power generation without attempting.
No matter use discharge gas that can all generate volume using which kind of technique, combustion exhaust gases or during production of energy Outer CO2Gas, and be discharged in air.In some areas, such as Europe, a large amount of CO are discharged2The industry of gas is according to it Use production CO2The raw material of gas levies taxes and/or is required to buy CO2Trading right, often make this production of energy process without Ji.
In order to reduce release to the greatest extent, CO can be captured2Gas simultaneously stores or is used for one or more industrial process.Citing comes Say exist CO2Gas is used as the industrial process of raw material.But these applications usually require the CO of concentration and high-purity2Gas. The example of these industrial process includes cement sectors, beverage industries (such as in production of soda), for by so-called dry Reforming process or the synthesis gas being combined with steam reformation generate, or with steam reformation and pass through so-called tri-reforming part oxygen Change or for by using H2Chemical conversion produces methanol.However, the CO generated in combustion2The concentration of gas and/or pure Degree is typically not enough to for use as the raw material in this kind of application.
CO in isolation discharge gas2The process of gas is usually also required to a degree of energy input, to generate ratio The more CO captured2.In other words, CO2Conversion and/or isolation processes are often thermodynamically unfavourable, this needs additional CO2The energy input of formation.For example, it is known that CO is absorbed by solution amine-based2For absorbing CO2Gas is that have very much Effect and selectivity.However, recycling CO from this kind of solution2Also referred to as regeneration step is highly endothermic.Therefore, it is this again Raw process needs energy, increases so as to cause additional energy expenditure and therefore CO2The discharge of gas.
Therefore, it is necessary to improve to reduce to contain CO and CO2CO in the discharge of gas2Discharge.
Invention content
The disclosure provides the CO for helping to reduce the discharge gas generated in industrial process2Discharge also generates valuable simultaneously Hydrocarbon raw material method and integrated system.The method includes：With chemical absorbent carbon dioxide is captured from first gas stream (CO2) gas, wherein first gas stream includes carbon monoxide (CO) gas and CO2Gas has to generate compared with first gas stream The CO gases of higher concentration and the CO of low concentration2The second gas stream of gas；With hydrogen (H2) and second gas stream in CO gas Body generates hydrocarbon from Fischer-Tropsch reaction (Fischer-Tropsch reaction), and wherein Fischer-Tropsch reaction generates heat；And it uses At least part heat generated in Fischer-Tropsch reaction is by discharging the CO captured from first gas stream2Gas regenerates chemical suction Receive agent.
The CO gases and CO of first gas stream2Molar ratio (the molal quantity of CO gases of gas:CO2The molal quantity of gas) be 0.5:1 to 10:1, wherein first gas stream can also have CO gases and CO2Gas (the molal quantity of CO gases:CO2Gas rubs That number) it is 0.5:1 to 2.5:1.It includes generating C to generate hydrocarbon from Fischer-Tropsch reaction5To C20Hydrocarbon, wherein coming from H2The H of gas source2Gas With for from Fischer-Tropsch reaction generate C5To C20CO gas in the second gas stream of hydrocarbon and H2Gas is with 1:1 to 3:H in 1 range2 Gas and CO gases (H2The molal quantity of gas:The molal quantity of CO gases) molar ratio reaction.As described above, Fischer-Tropsch reaction is produced A part for heat amount, the heat can be used for by discharging the CO captured from first gas stream2Gas regenerates chemical suction Receive agent.The heat generated during Fischer-Tropsch reaction can also be used for generating electricity, wherein the waste heat to generate electricity is used as generating during Fischer-Tropsch reaction Heat part to regenerate chemical absorbent.
Especially, the integrated system of the disclosure includes：CO2Absorption system, the CO2Absorption system has at least having There are CO gases and CO2The entrance of the first gas stream of gas, wherein the CO2Absorption system utilizes chemical absorbent from the first gas Body stream captures CO2Gas, to generate the CO of CO gases and low concentration with higher concentration compared with first gas stream2Gas Second gas stream；It is connected to hydrogen (H2) source and it is connected to CO2Absorption system to receive the fischer-tropsch reactor of second gas stream, The wherein described fischer-tropsch reactor is used to be catalyzed the hydrocarbon generated from Fischer-Tropsch reaction and comes from the H2Gas source and from described The CO gases and H of second gas stream2Gas, wherein the Fischer-Tropsch reaction generates heat；Fischer-tropsch reactor is connected to capture The heat exchanger of the heat generated during Fischer-Tropsch reaction；And it is connected to CO2The CO of absorption system and heat exchanger2Desorption system System, wherein at least part hot recycling CO of the heat captured by the heat exchanger for being connected to fischer-tropsch reactor2In desorption system Chemical absorbent to discharge the CO of capture2Gas.Fischer-tropsch reactor can within the scope of 200 DEG C to 260 DEG C temperature and It is operated together with Co catalysts under pressure in 0.5Mpa to 5MPa ranges.In another embodiment, by the heat of fischer-tropsch reactor The heat of exchanger capture is initially used for generating electricity, wherein remaining waste heat is used for hot recycling CO after power generation2In desorption system Chemical absorbent.
Description of the drawings
Fig. 1 provides the diagram of the integrated system according to the disclosure.
Fig. 2 provides the diagram of the integrated system according to the disclosure.
Specific implementation mode
The concern for leading to the greenhouse gases anthropogenic discharge of harmful climate change is being increased.Carbon dioxide (CO2) by It is determined as one of main greenhouse gas, and is for example discharged in the discharge gas of industrial process.This kind of industrial process include but It is not limited to fossil fuel energy facility, steel-making facility, biomass energy facility, natural gas processing facility, synthetic fuel power plant, refining Oily factory, petrochemical iy produced factory and fossil fuel hydrogen preparation plants.In some cases, these exhaust gas also contain CO, such as in steel It is particularly the case in the exhaust gas of ironworker's industry.Before being discharged into the atmosphere, due to its toxicity, the CO gases in exhaust gas need to turn Turn to CO2Gas.Combustion process can be used for generating CO2Gas and the heat that can be used for various processes.
CO is discharged in order to prevent2Gas, it has been proposed that various capture techniques.In these capture techniques, it is believed that chemistry It absorbs and is most suitable for capturing CO from the discharge gas of these industrial process2Gas.However, chemical absorbing needs energy to regenerate Rich in CO2Chemical absorbent.In general, the energy needed for regeneration chemical absorbent also will produce CO2Gas, this can reduce capture CO2The whole efficiency and validity of gas.
In order to solve this problem, disclosure providing method and integrated system, the method and integrated system help to subtract The CO of the discharge gas generated in few industrial process2Discharge, while also generating and can substitute carbon-based product (i.e. stone from fossil sources Oil or natural gas) valuable hydrocarbon products.The method and integrated system being discussed herein utilize chemical absorbent from first gas stream Capture CO2Gas, to generate the CO of CO gases and low concentration with higher concentration compared with first gas stream2The of gas Two gas streams.CO gases in second gas stream and hydrogen (H2) be used to produce hydrocarbon in Fischer-Tropsch reaction together.Hydrocarbon forms essence On save CO2The discharge of gas because CO gases are converted into valuable product, rather than undergo burning and generates more CO2 Gas.The CO that at least part heat generated in Fischer-Tropsch reaction is used to capture from first gas stream using release2Gas is again It is raw to be rich in CO2Chemical absorbent.The heat captured during Fischer-Tropsch reaction can also optionally be initially used for generating electricity, wherein Remaining heat is subsequently used for hot recycling and is rich in CO after power generation2Chemical absorbent.Therefore, the disclosure unexpectedly provides From generally the waste stream containing CO generates valuable hydrocarbon by waste, while CO is captured under the input of low net energy2Gas.
As used herein, term " discharge gas (effluent gas/effluent gases) " refers to any at least wrapping Containing CO2The post-treatment gas of gas and CO gases.The example of one or more discharge gases includes flue gas, exhaust gas, discharge gas And/or the process gas from industrial process, as those described herein.
As used herein, " pipeline " associated with integrated system indicates pipeline or conduit with sufficient size, and And with the suitable material of the fluid (such as liquid or gas) for conveying instruction in-line movement.It should be understood that for moving The one or more pumps and/or compressor of dynamic fluid or other known device also with the pipeline of integrated system discussed in this article and Component is associated.However, this kind of equipment is not shown, to allow diagram preferably to show the disclosure.It is shown in the figure of integrated system In arrow on " line " indicate the direction of fluid flowing.
As used herein, " one (a/an) ", " described ", " at least one/kind " and " one or more/one or more " It is used interchangeably.Term "comprising", " comprising " and its variant its appearance in the specification and in the claims in the case of all Without restrictive, sense.Term "and/or" refers to one in listed element, is more than one or all.As used herein, Term " about " can be not limited to specified exact value.In at least one example, it can be come with the accuracy of reference measure instrument true Determine the variance represented by term " about ".Also in this context, include institute in the range by the narration of endpoint logarithm range Including all numbers (such as 1 to 5 include 1,1.5,2,2.75,3,3.80,4,5 etc.).
The disclosure it is described in detail below in, with reference to forming part thereof of attached drawing, and pass through diagram in the accompanying drawings Mode show can how one or more embodiment of the disclosure.These embodiments are described in detail enough so that ability The those of ordinary skill in domain can embodiment of the disclosure and can and it should be understood that other embodiments can be utilized Changed with carrying out technique, chemistry and/or structure in the case where deviateing the scope of the present disclosure.
Attached drawing herein follows numbering convention, wherein the first bit digital corresponds to accompanying drawing number, and remaining number mark Know the element or component in attached drawing.Similar components or component between difference diagram can be known by using similar number Not.For example, 110 can be with the element " 10 " in reference chart 1, and similar element can be with 210 in reference chart 2.As incited somebody to action Understand, element shown in various embodiments herein can be added, exchanges and/or eliminate, in order to provide the multiple of the disclosure Additional examples of composition.In addition, as will be appreciated, the ratio and relative scale of the element provided in attached drawing are intended to illustrate the implementation of the present invention Example, and be not be considered in a limiting sense.
Referring now to Figure 1, embodiment of the explanation according to the integrated system 100 of the disclosure.Integrated system 100 includes two masters Process, the main process is wanted to integrate as follows：Both chemical absorbent was used to capture CO2Gas again use in exothermic process The heat hot recycling chemical absorbent captured in (such as fischer-tropsch reaction), the exothermic process is by CO gases and H2Gas is converted into Hydrocarbon.As shown in fig. 1, integrated system 100 includes CO2Absorption system 102, the CO2Absorption system 102 uses chemical absorbent Operation is to absorb the CO from first gas stream 1042Gas, thus generate has higher concentration compared with first gas stream 104 CO gases and low concentration CO2The second gas stream 106 of gas.As will be more discussed fully herein, second gas stream 106 For in fischer-tropsch reactor 108, CO gases wherein in second gas stream 106 with come from second gas stream 106 and logistics 138 The H of the two2Gas reaction is to generate the hydrocarbon and heat from heat release Fischer-Tropsch reaction.As will be described herein, in Fischer-Tropsch reaction The heat generated in device 108 is for regenerating CO2Chemical absorbent in desorption system 110.
It can be used for CO there are a variety of2Absorption system 102 and CO2The CO of desorption system 1102Gas entrapment technology.This kind of CO2 Gas entrapment technology may include that physical absorption, physical absorption, membrane technology and/or chemical absorbing come from first gas stream to capture 104 CO2Gas.In these techniques, it is preferable to use chemical absorbent carries out chemical absorbing, because it is best suited for retouching herein CO present in the exhaust gas for the industrial process stated2The volume of gas, pressure and temperature.However, as described above, using chemical absorbing Agent brings some disadvantages, and most significant is it in CO2The high energy in regeneration in desorption system.Disclosure usage charges- Tropsch reactors 108 provide at least necessary energy to regenerate CO2Chemical absorbent in desorption system 110.
As shown in fig. 1, CO2Absorption system 102 includes for capturing CO from first gas stream 104 using chemical absorbent2 The absorption tower 112 (also referred to as washer or absorber) of gas.Fig. 1 also illustrates CO2Desorption system 110 has for regenerating Chemical absorbent simultaneously discharges the CO captured from first gas stream 1042The desorber 114 (also referred to as stripper) of gas.CO2It absorbs System 102 and CO2Desorption system 110 is used to capture CO from first gas stream 104 using the chemical absorbent in absorption tower 1122Gas Body, to generate the CO of CO gases and low concentration with higher concentration compared with first gas stream 1042Second gas of gas Body stream 106.
Multiple compounds and its solution can be used for chemical absorbent.For example, chemical absorbent can be amine-based Compound.The specific example of this kind of compound amine-based can include but is not limited to amine, alkanolamine, ionic liquid and/or Piperazine.Preferably, alkanolamine can include but is not limited to the primary, secondary and/or tertiary amine containing at least one OH and amido.This The example of class alkanolamine includes selected from the group being made up of：Monoethanolamine (MEA), 2- dipropanolamines (DIPA), diethyl Hydramine (DEA), triethanolamine (TEA), N methyldiethanol amine (MDEA), diglycolamine (DGA), 2- amino-2-methyls -1- third Alcohol (AMP) with and combinations thereof.
Preferably, using aqueous alkanolamine solution as CO2Chemical absorbent in absorption system 102.Alkanol aqueous amine Solution includes the solution of one or more alkanolamines provided herein and water.Preferably, with the gross weight of aqueous alkanolamine solution Gauge, CO2Aqueous alkanolamine solution used in absorption system 102 has the concentration that 20 weight % (wt.%) arrive 55wt.%. Finally, due to which the various characteristics and advantage of various chemical absorbents provided herein, can also use two or more chemistry CO in the mixture enhancing absorption tower 112 of absorbent2Gas entrapment efficiency.
As understood by those skilled in the art, the volume of first gas stream 104, composition, CO2Concentration, temperature and other Parameter aids in determining whether the function of each, configuration, quantity, size and operating parameter in absorption tower 112 and desorption column 114. In general, absorption tower 112 can in the range of the pressure of about 100kPa and 40 DEG C to 60 DEG C at a temperature of operate.Alternatively, Absorption tower 112 can operate under the pressure in 5kPa to 8400kPa ranges, and temperature range is 15 DEG C to 65 DEG C.Absorption tower 112 Specific example operating pressure can also include 500kPa to 4000kPa, temperature range be 25 DEG C to 50 DEG C.Operate absorption tower 112 definite pressure and temperature can depend on the exact composition of used chemical absorbent.Desorber 114 can be about The pressure of 100kPa and in the range of 90 DEG C to 135 DEG C at a temperature of operate.Alternatively, desorber 114 can be arrived in 100kPa It is operated under pressure within the scope of 250kPa, temperature range is 90 DEG C to 110 DEG C.The specific example operating pressure of desorber 114 is also May include 40kPa to 170kPa, temperature range is 90 DEG C to 110 DEG C.Similarly, it is hobbed really for operating desorber 114 Power and temperature can again depend on the used exact composition of chemical absorbent, the thermal stability of chemical absorbent and molten The rich carrying capacity of agent.It should be understood that the volume flow etc. of gas to be treated is depended on, in absorption tower 112 and/or desorber 114 Each in two or more can be used for CO2In absorption system 102.
The example on absorption tower 112 may include configuration be plate column, packed bed, spray tower, bubble tower or spray tower that A bit.In order to exchange CO between liquid and gas2Gas, absorption tower 112 can be relative to first gas stream 104 and chemical absorbings Agent is with reflux type operates simultaneously or preferably.Thus, for example, as shown, first gas stream 104 can be existed by pipeline 118 Enter the bottom on absorption tower 112 at entrance 116, and with chemical absorbent counter current contacting.Inside absorption tower 112, first gas CO in stream 1042Gas is transferred to chemical absorbent liquid phase from gas phase.The CO of chemical absorbing liquid phase is transferred to from gas phase2Gas Amount is number of trays in absorption tower 112 or can use the function of filler height, for given its size of situation and configuration at this Within the scope of field technology.The CO of chemical absorbing liquid phase is transferred to from gas phase2The amount of gas is also concentration of absorbing, liquid-gas ratio and behaviour Make the function of temperature and pressure.
Rich in CO2Chemical absorbent taken out and sent to CO by pipeline 120 in the lower part on absorption tower 1122Desorption system 110 desorber 114 is regenerated.The example of desorber 114 may include being configured to packed bed tower, plate column, spray tower or drum Those of bubble column.Rich in CO2Chemical absorbent via pipeline 122 enter desorber 114 near top.As shown, CO2 Desorption system 110 includes the reboiler 124 for heat to be introduced to desorber 114.Reboiler 124 contributes to heating to be rich in CO2 Chemical absorbent to discharge the CO of absorption2Gas, to make chemical absorbent in its approach by desorber 114 again It is raw.
The CO of release2Gas forms bubble, when the bubble rises to the top of desorber 114, the bubble and change Learn absorbent reverse movement.The CO of release2Gas can be contributed to by condenser 126 in CO2CO of the gas as recycling2 Gas stream 128 leaves CO2Water removal and other compounds are gone before desorption system 110.The CO of recycling2Gas stream 128 is containing relatively high The CO of concentration2Gas.For example, with the CO of recycling2The total volume meter of gas stream 128, the CO of recycling2Gas stream 128 can contain There is the CO of at least 95 volume %2Gas.The CO of recycling2Gas stream 128 can be used for one or more industrial process or storage.
Regenerated chemical absorbent is removed via pipeline 130 from the lower part of desorber 114.Chemical absorbing in pipeline 130 Agent then may pass through heat exchanger 132.Heat exchanger 132 allows the heat transfer in the chemical absorbent in pipeline 130 to arrive Rich in CO2Chemical absorbent, it is described be rich in CO2Chemical absorbent be transported to CO at it2The desorber of desorption system 110 It is taken out in the lower part on absorption tower 112 via pipeline 120 before 114.Chemistry in heat exchanger 132 in cooling pipeline 130 Then absorbent is introduced back into the top on absorption tower 112 by pipeline 134, to make in new cycle as chemical absorbent With.In general, before entering absorption tower 112, stream 134 is further cooled down using lean amine cooler first.
Referring again to CO2Absorption system 102, first gas stream 104 enter CO at entrance 1162The suction of absorption system 102 Receive tower 112.Depending on its composition, first gas stream 104 can directly be used from its source (that is, directly from industrial process Gas is discharged).Alternatively, first gas steam 104 derives from the discharge gas by discharge gas treating process 136, the gas Body processing procedure 136 includes one or more of a series of chemical processes and/or washer, to remove or reduce discharge gas One or more components percent by volume.For example, first gas stream 104 may include solid particle (such as dust Particle and/or soot particulates), wherein discharge gas treating process 136 may include electrostatic precipitator, cyclone separator and/or Fabric filter, with removal from CO2First gas stream 104 in absorption system 102 captures CO2Before gas, the first gas is come from At least part solid particle of body stream 104.
In addition, in CO2CO is captured in absorption system 1022Before gas, operable discharge gas treating process 136 is with from The capture of one gas stream 104 is at least one additional material of gas phase.The example of this kind of additional material includes having selected from amine, vulcanization Close those of object, phosphate and the part of cyanide group substance.Thus, for example, waste gas treatment process 136 may include discharge Gas sweetening is to capture and remove SOxGas is (for example, SO2Gas and SO3Gas).The nitrogen oxides in gas is discharged (if deposited If) it can be reacted by high temperature in gas treating process 136 is discharged or with the catalysis of ammonia or urea to handle, by NOx Gas is converted into N2Gas.As it is known, hydrogen sulfide (if present) can use amine or caustic alkali washing process to make a return journey It removes.Cyanide can be by hydrolysis at amine (NH3), then removed in absorption step.Caustic solution (such as hydroxide Sodium solution) it can also be used for helping to remove cyanide from first gas stream 104.During discharge gas treating process 136, discharge Other components of gas, as mercury, arsenic or other metals (if present) can for example by the absorption of absorbent or pass through Capture is removed as discharge gas sweetening product from discharge gas in inert solid.As discussed herein, in discharge gas The selection for the process that body processing procedure 136 includes can be at least partially based on the type of the discharge gas received from industrial process With composition and the expectation based on first gas stream 104 forms.For specific other compounds in discharge gas, by that will arrange Removal can also be realized by going out gas and being exposed to chemicals present in absorbers combination.However, these absorptions may influence to absorb The operational efficiency of system.
Preferably, in terms of the total volume percent of first gas stream 104, first gas stream 104 has at least 20 volumes hundred Divide than (volume %) CO gases and CO2The combined amount of gas.About each component, first gas stream 104 includes 5 to 80 volumes hundred Divide the nitrogen (N than (volume %)2), 15 to 80 volume %CO gases, 5 to 40 volume %CO2Gas and 1 to 60 volume % hydrogen (H2).Preferably, first gas stream 104 includes 5 to 60 volume %N2Gas, 15 to 50 volume %CO gases, 5 to 35 volume % CO2Gas and 1 to 35 volume %H2Gas.Most preferably, first gas stream 104 includes 5 to 50 volume %N2Gas, 15 to 35 Volume %CO gases, 5 to 25 volume %CO2Gas and 1 to 10 volume %H2Gas.Given volume percent value first gas stream 104 always add up to 100 volume % with the total volume meter of first gas stream, the wherein percent by volume of first gas stream 104.This The first gas logistics that text discusses can also include other components, and the percent by volume of wherein first gas logistics 104 is always total It is calculated as 100 volume %.The example of other components can include but is not limited to gaseous methane, oxygen and argon gas and send out in an atmosphere Existing other gases.
Other than above-mentioned percent by volume, surprisingly, it was found that CO gases and CO2Certain molar ratios of gas allow The energy generated in fischer-tropsch reactor 108 and operation CO2Reach at least minimum energy between energy needed for desorption system 110 Amount balance.For example, by carefully balancing the energy generated in fischer-tropsch reactor 108 and operation CO2110 institute of desorption system The energy needed, as CO gases and CO2Gas mole ratio is at least 0.5:When 1, energy neutral can be obtained from first gas stream 104 Or relatively low energy-intensive technique.Preferably, the composition of first gas steam 104 has 0.5:1 to 10:1 CO gases and CO2 Molar ratio (the molal quantity of CO gases of gas:CO2The molal quantity of gas).It is highly preferred that first gas stream 104 can have 0.5:1 to 5:1 CO gases and CO2The molar ratio of gas.Most preferably, first gas stream 104 can have 0.5:1 to 2.5: 1 CO gases and CO2The molar ratio of gas.
Into CO2The first gas stream 104 of absorption system 102 can be with the temperature within the scope of 5 DEG C to 100 DEG C.Preferably, The temperature of first gas stream is in the range of 15 DEG C to 65 DEG C.It is highly preferred that the temperature of first gas stream is at 25 DEG C to 50 DEG C In range.Into CO2The first gas stream 104 of absorption system 102 can have the pressure in 5kPa to 8400kPa ranges.It is excellent Selection of land, first gas stream 104 have the pressure in 500kPa to 5000kPa ranges.It is highly preferred that first gas stream 104 has There is the pressure in 1500kPa to 3000kPa ranges.
As shown in Figure 1, CO2Desorption system 110 is connected to CO2Both absorption system 102 and fischer-tropsch reactor 108.Fischer-Tropsch Reactor 108 is also connected to hydrogen (H via pipeline 1382) source, and it is connected to CO2Absorption system 102 at entrance 140 to connect Receive second gas stream 106.As discussed herein, fischer-tropsch reactor 108 is used for from H2The H of gas source2Gas (logistics 138) With the CO gas and H in second gas stream 1062Gas is catalyzed by Fischer-Tropsch reaction generates hydrocarbon, and wherein fischer-tropsch reaction generates hydrocarbon and heat (i.e. heat release).Preferably, as discussed herein, it includes generating C to generate hydrocarbon from Fischer-Tropsch reaction5To C20Hydrocarbon.
In general, fischer-tropsch reactor 108 is for allowing CO gases and H from second gas stream 1062Gas and From H2The H of gas source (logistics 138)2Gas carries out Fischer-Tropsch reaction to generate hydrocarbon in a series of exothermic reactions.Such as this field Technical staff is understood that Fischer-Tropsch reaction is series reaction, gives selected reactor design, operating condition (such as CO:H2 Gas ratio, flow velocity, reaction temperature and pressure), including the catalyst of carrier material and one or more accelerating agents and other Factor generates the mixture of hydrocarbon.In a preferred embodiment, under suitably selection Fischer-Tropsch catalyst and process conditions, have There may be hydrocarbon, the hydrocarbon includes at least hydrocarbon of the carbon chain lengths of 50 weight % between 5 or higher and 20 or lower, wherein carbon The score of ranging from 21 or higher hydrocarbon is less than 10 weight %, preferably smaller than 5 weight %.These hydrocarbon products are preferably straight chain Hydrocarbon, such as normal alkane and/or positive alkene.As understood by those skilled in the art, the selection of catalyst and process conditions can be used Optimize and/or adjust required product, such as to minimize the yield of methane and make C5To C20The maximum production of hydrocarbon-fraction, And/or linear/branch's ratio is made to maximize.
Hydrogen molar concentration in first gas stream is usually less than the CO molar concentrations in this phase cocurrent flow, leads to H2Mole with CO molar ratios are less than 1:1.Increase H known to those skilled in the art2Method mole with CO molar ratios.For example, can make With water-gas shift reactor by CO and H2O is converted to CO2And H2, to increase H2Mole with CO molar ratios.It is preferable, however, that choosing Ground hydrogen source is selected to produce useful chemicals using CO to the maximum extent.This additional H2Gas can be used as logistics 138 Fischer-tropsch reactor 108 is supplied, by H2:CO ratios increase to the desired ratio of Fischer-Tropsch reaction.
The design of fischer-tropsch reactor 108 can be selected from several reactor designs, and the reactor design includes multitube Formula fixed bed reactors, fluidized-bed reactor, slurry reactor and fluid bed and recycling catalyst reactor.Depending on reactor Design, fischer-tropsch reactor 108 can operate at a temperature in the range of 150 DEG C to 500 DEG C.Preferably, fischer-tropsch reactor 108 Operation temperature can be in the range of 150 DEG C to 300 DEG C.The operating pressure of fischer-tropsch reactor 108 can arrive for 100kPa 10000kPa.Preferably, the operating pressure of fischer-tropsch reactor 108 can be in the range of 1000kPa to 5000kPa.It is various to urge Agent can be used for fischer-tropsch process.The example of suitable catalyst includes but not limited to cobalt, iron and/or ruthenium.It is preferable to use cobalt catalysis Agent.For example, it is used for selectively formed C5To C20The suitable cobalt-base catalyst and processing conditions of hydrocarbon-fraction can be found in What September in 2015 was submitted on the 21st《Form normal alkane (Forming Normal Alkanes)》(international application no PCT/US15/ 51189) it is submitted within 21st with September in 2015《Form light hydrocarbon (Forming Light Hydrocarbons)》(international application Number PCT/US15/51234), full contents of the two applications are incorporated herein by reference.
Catalyst can also include carrier, such as silica, aluminium oxide, titanium dioxide and/or zeolite.Accelerating agent can also It is used together with catalyst, the example of wherein accelerating agent includes but not limited to potassium and copper compound, as known in the art.Accelerating agent Selection may depend on selected catalyst and hydrocarbon to be generated.In addition, the selection of the operation temperature and pressure of Fischer-Tropsch reaction Depending on various factors, including reactor design, hydrocarbon to be produced, catalyst and the catalyst used in Fischer-Tropsch reaction and Catalyst load value.
As discussed herein, CO2Absorption system 102 is used to absorb CO from first gas stream 104 using chemical absorbent2Gas Thus body generates the CO of CO gases and lower concentration with higher concentration compared with first gas stream 1042Second gas of gas Body stream 106.Preferably, CO2Absorption system 102 is for recycling at least 90 percent by volume (bodies present in first gas stream 104 Product %) to the CO of 95 volume %2Gas.In other words, CO can be selected2One or more chemical absorbings of absorption system 102 Agent, the selection of operation temperature and/or operating pressure remove at least 90 volume % to 95 bodies will pass through from first gas stream 104 The CO of product %2Gas forms second gas stream 106.CO of the removal more than 95 volume % from first gas stream 1042Gas It is possible.
In view of at least 90 volume % to 95 volume % are removed from first gas stream 104 when producing second gas stream 106 CO2Gas, CO gases and CO in second gas stream 1062The molar ratio of gas will be greater than first gas stream 104.Citing comes It says, the CO gases in second gas stream 106 and CO2The molar ratio of gas can be 5:1 to 200:1 (the molal quantity of CO gases:CO2 The molal quantity of gas).Preferably, the CO gases and CO in second gas stream 1062The molar ratio of gas can be 10:1 to 100: 1 (the molal quantity of CO gases:CO2The molal quantity of gas).
Use the H by pipeline 138 and the supply of second gas stream 1062Gas, fischer-tropsch process can be in fischer-tropsch reactor With 0.1 in 108:1 to 10:1 H2The molal quantity of gas:The mole ratio of CO gases carries out.Preferably, it is used for anti-in Fischer-Tropsch Answer the middle H for generating hydrocarbon2Gas and CO gases 106 are with 1:1 to 3:H in 1 range2Gas and CO gases (H2The molal quantity of gas:CO The molal quantity of gas) molar ratio reaction.H2The gas hourly space velocity of gas and CO gases under given molar ratio can be 100hr-1To 10000hr-1In range.In a particularly preferred example, fischer-tropsch reactor is together with Co catalysts at 200 DEG C It is operated under the pressure in temperature and 1000kPa to 5000kPa ranges within the scope of to 260 DEG C, wherein H2The H of gas and CO gas2Gas Molar ratio (the H of body and CO gases2The molal quantity of gas:The molal quantity of CO gases) it is 1:1 to 3:1.This particularly preferred reality Example allows H2Gas and CO gases generate C from Fischer-Tropsch reaction5To C20Hydrocarbon.
It is supplied to the H of the fischer-tropsch reactor 108 in second gas stream 1062Gas, which comes from, to be present in first gas stream 104 H2Gas.The H of fischer-tropsch reactor 108 is supplied to by pipeline 1382Gas can come from any amount of hydrogen gas production work Skill.H2The example of gas source may include the oven gas from steelmaker, the hydrogen byproduct stream from dehydrogenation unit, steam Process, oil refining process come from steam reforming process or electrolysis process.As known in the art, integrated system 100 can be with Further comprise H2Gas cleaning processes 142, selection depend on H2Gas source.H2Step in gas cleaning processes 142 is shown Example can include but is not limited to one or more of a series of chemical technologies and/or washer to remove or reduce H2Gas The percent by volume of one or more components.For example, electrostatic precipitator, cyclone separator and/or fabric mistake can be used Filter is present in H to remove2At least part of any solid particle in gas stream 138.Other technologies, such as pressure-variable adsorption, It can be used to clean H as needed2Gas stream 138.Thus, for example, H2Gas-treating processes 142 may include that discharge gas is de- Sulphur is to capture and remove pollutant containing S.As it is known that hydrogen sulfide (if present) can use amine or caustic alkali washing process To remove.Ammonia (NH3) can be removed by washing process or absorption process.Cyanide can be by hydrolysis at amine (NH3), Then removed in absorption step.Caustic solution (such as sodium hydroxide solution) can also be used for helping from first gas stream 104 Middle removal cyanide.During discharge gas treating process 142, other components such as metal (if present) of gas is discharged A part for discharge gas sweetening product can be for example used as by adsorbing on the sorbent or by being captured in inert solid It is removed from discharge gas.As discussed herein, the selection for being included in the process in discharge gas treating process 142 can at least portion Divide the expectation composition of type and composition and first gas stream 104 based on the discharge gas received from industrial process.In a tool In body embodiment, additional H2Source gas can be co-fed to purification part 136 with first gas stream 104 and via CO2It inhales Receipts system 102 is fed to fischer-tropsch reactor 108.Additional H from another source2Gas still may be needed as stream 138 Fischer-tropsch reactor 108 is fed to realize desired H2:CO gas ratios are to carry out Fischer-Tropsch reaction.
The output of fischer-tropsch reactor 108 is transported to separative element 144, from Fischer-Tropsch reaction in separative element 144 The hydrocarbon of generation and CO gases, H2Gas, CO2It is detached in the gases such as gas and vapor.Other than other selections, separative element 144 can be traditional gas-liquid separator, and the gas-liquid separator application condensation principle is at reduced temperatures to produce condensation Object is detached with gaseous products.
In one embodiment, if it is desired, the product liquid from separative element 144 can be further processed so that Product is suitble to desired specification.It cracks if desired, this kind of unit operation may include catalyzed conversion such as (water) and/or adds hydrogen de- Oxygen is with cracking and/or isomerization product and removes the oxygenatedchemicals formed in Fischer-Tropsch reaction sometimes.
Optionally, what is detached from fischer-tropsch reactor 108 and in separative element 144 contains CO2Gas can pass through pipeline 146 are supplied to CO2The entrance 116 of absorption system 102 with chemical absorbent to be captured.In addition, pipeline 147 can be used for Fischer-Tropsch Remaining at least part CO gases and H after reaction2Gas returns to fischer-tropsch reactor 108.As shown, pipeline 147 can be Second gas stream 106 is added before into fischer-tropsch reactor 108.
Fischer-tropsch reactor 108 may further include heat exchanger 148 and be generated in the process extremely with capturing Fischer-Tropsch reaction Few a part of heat.In addition to other designs, heat exchanger 148 may include configuring in the design of fischer-tropsch reactor 108 Shell and tube heat exchanger.The heat generated during Fischer-Tropsch reaction is absorbed by the cooling fluid of heat exchanger 148, to help to protect Hold the reaction condition in fischer-tropsch reactor 108.The cooling fluid used in heat exchanger 148 may include water and other Known cooling fluid.
As shown in Figure 1, CO2Desorption system 110 is connected to heat exchanger 148.Specifically, CO2Desorption system 110 is again Boiling device 124 is connected to heat exchanger 148 by pipeline 150.The cooling fluid used in heat exchanger 148 is absorbed in Fischer-Tropsch The heat generated during reaction, wherein then the cooling fluid is supplied to CO by pipeline 1502Desorption system 110 boils again Device 124 so that generated in Fischer-Tropsch reaction and at least part of heat for being captured by heat exchanger 148 then can be with For making the chemical absorbent hot recycling in desorption system 110 to discharge the CO captured from first gas stream2Gas.
As shown in Figure 1, carrying out the cooling fluid of automatic heat-exchanger 148 after the heat generated during absorbing Fischer-Tropsch reaction Enter reboiler 124 at entrance 152, reboiler 124 will be in the cooling fluid from heat exchanger 148 at entrance 152 This heat be transported in desorber 114 be rich in CO2Chemical absorbent.As described herein, heat then allow from rich in CO2Chemical absorbent in discharge the CO of absorption2Gas, to make chemical absorbent in the approach by desorption column 114 again It is raw.
Referring now to Figure 2, another embodiment of the displaying according to the integrated system 200 of the disclosure.As shown, integrated system 200 include two main process previously in conjunction with Fig. 1 discussion, and two of which main process integrates as follows：Both useization It learns absorbent and captures CO2Gas keeps chemical absorbent hot using the heat captured in exothermic process (such as Fischer-Tropsch reaction) again Regeneration, the exothermic process is by CO gases and H2Gas is converted into hydrocarbon.For brevity, the discussion of component shown in Fig. 1 is herein It is not repeated, but is shown in FIG. 2 and is attached in the discussion of following figure 2 at this.
Fig. 2 shows the embodiment of the disclosure that energy " transfer " occurs wherein between three main process.Such as preceding institute It states, the two main process integrate as follows：Both chemical absorbent was used to capture CO2Gas again use in exothermic process Heat (such as fischer-tropsch reaction) hot recycling chemical absorbent of capture, the exothermic process is by CO gases and H2Gas is converted into Hydrocarbon.Fig. 2 integrates power generating process (for example, electric energy generating equipment based on steam) now, preferably by anti-from Fischer-Tropsch The heat answered by boiler feedwater to be preheating to power generating process first.This allows power generating process keeping identical electric energy Its fuel usage amount is reduced while output.
As shown in Fig. 2, integrated system 200 includes power generating process 254.Various power generating process be it is known, with Under be only one example.It will be appreciated that can not change present disclosure in the case of being generally understood by other known group Part replaces and/or is added to power generating process 254.
Except it is as known in the art it is other in addition to, power generating process 254 includes：Steam turbine 256, via the machinery of axis 260 Ground is connected to the generator 258 of steam turbine 256, to allow the mechanical energy from steam turbine 256 to be converted into electric energy, can pass through Electric wire 262 is transported to external circuit.264 heating boiler feed water of stove is to be produced as the high steam of the energy supply of steam turbine 256.Stove 264 The fuels such as coal conveyed by pipeline 266, fuel oil, natural gas or shale oil can be used to operate.By what is generated by stove 264 High steam is supplied to steam turbine 256 at entrance 268, and being provided in 256 mesohigh steam of the steam turbine makes the rotation of axis 260 Work(.
For the third process is connected to be discussed above two processes, heat associated with fischer-tropsch reactor 208 is handed over Parallel operation 248 is connect with power generating process 254.Specifically, the stove 264 of power generating process 254 is connected to by pipeline 250 Heat exchanger 248.Heat-exchange fluid (such as hot water condensate) in pipeline 250 is pumped after being heated in heat exchanger 248 It is sent to the entrance 270 of stove 264.Here, heat-exchange fluid can enter stove 264 as a part for boiler feedwater.Alternatively, can make With heat exchanger by the heat transfer of the heat-exchange fluid from heat exchanger associated with fischer-tropsch reactor 208 248 to head First preboiler water supply.The discharge gas 282 generated by stove 256 can be recycled and returned to so that CO is added2The of absorption system 202 One gas stream 204.
Therefore, the heat for being generated and being captured by the heat exchanger 248 in fischer-tropsch reactor 208 during Fischer-Tropsch reaction is first It is first used to generate electricity.This allows the heat-exchange fluid of the heat exchanger 248 from fischer-tropsch reactor 208 first in electric energy production mistake It is used with high-energy gesture in journey 254.As discussed herein, remaining waste heat will subsequently function as in Fischer-Tropsch reaction after power generation A part for the heat generated in journey is with the CO of hot recycling integrated system 2002Chemical absorbent in desorption system 210.Herein In the process, about 50% can be increased to from about 40% by calculating the efficiency of power generating process, with the 1.1kT/ per 1MW power Y/ or 3.7T CO2The related CO for the product that/T is generated2It reduces.
As shown, steam turbine 256 has the outlet for steam, the position of middle outlet is configured for specific mesh 's.As shown, steam turbine 256 is left in exhaust steam outlet 272, the exhaust steam in pipeline 274 is supplied to condenser 276, the condenser 276 condenses and returns to condensate through pipeline 278 entrance 270 of stove 264, to regenerate high pressure steaming Vapour.Steam turbine 256 is further equipped with side outlet port 280, and the outlet port 280 provides the reboiler 224 suitable for desorber 214 Steam under temperature and pressure is rich in CO to heat2Chemical absorbent to discharge the CO of absorption2Thus gas is passing through solution It inhales and regenerates chemical absorbent in the approach of column 214.Then the condensate from reboiler 224 can be returned to heat exchanger 248 entrance 252.As discussed herein, the heat for the waste heat that this permission would generally become steam turbine 256 is currently used for regenerating For capturing CO2The chemical absorbent of gas, the heat can enter air in other ways.Therefore, this configuration provides Improved energy uses layered structure, wherein the heat not only generated in fischer-tropsch reactor 208 is initially used for helping to generate electricity, also uses In regeneration for capturing CO2The chemical absorbent of gas.Effectively use doubles for this, and therefore makes in fischer-tropsch reactor 208 The calorie value of generation doubles.Therefore, having saved the energy, (dedicated energy production is CO2Another source of discharge) and capture CO2Gas.
The process for the integrated system 100 and/or 200 being discussed herein can be with batch process, semi-continuous process or continuous process It operates to operate.Preferably, the process for the integrated system 100 and/or 200 being discussed herein is operated with continuous process operation.

Claims (20)

1. a kind of method, including：
With chemical absorbent carbon dioxide (CO is captured from first gas stream2) gas, wherein the first gas stream includes an oxidation Carbon (CO) gas and CO2Gas, to generate the CO of CO gases and low concentration with higher concentration compared with first gas stream2 The second gas stream of gas；
With hydrogen (H2) and the second gas stream in the CO gases from Fischer-Tropsch reaction (Fischer-Tropsch Reaction hydrocarbon) is generated, wherein the Fischer-Tropsch reaction generates heat；And
Using at least part of the heat generated in the Fischer-Tropsch reaction, caught by discharging from the first gas stream The CO obtained2Gas regenerates the chemical absorbent.
2. according to the method described in claim 1, wherein in terms of the total volume percent of the first gas stream, first gas Body stream has the CO gases and CO of at least 20 percents by volume (volume %)2The combined amount of gas.
3. according to any method of the preceding claims, wherein the CO gases of the first gas stream with it is described CO2Molar ratio (the molal quantity of CO gases of gas:CO2The molal quantity of gas) it is 0.5:1 to 10:1.
4. according to the method described in claim 3, the CO gases of the wherein described first gas stream and the CO2Gas rubs You are than (the molal quantity of CO gases:CO2The molal quantity of gas) it is 0.5:1 to 2.5:1.
5. according to any method of the preceding claims, wherein capturing CO from the first gas stream2Gas is further Including at least one of capture gas phase other materials, wherein the substance has the group selected from amine, sulphur, phosphate and cyanide The part of group.
6. according to any method of the preceding claims, wherein it includes generating C to generate hydrocarbon from the Fischer-Tropsch reaction5It arrives C20Hydrocarbon.
7. according to the method described in claim 6, being wherein used to generate the C from the Fischer-Tropsch reaction5To C20The H of hydrocarbon2 The CO gases in gas and the second gas stream are with 1:1 to 3:H in the range of 12The molar ratio of gas and CO gases (H2The molal quantity of gas:The molal quantity of CO gases) reaction.
8. the method according to any one of claim 6 to 7, further comprising will be remaining after the Fischer-Tropsch reaction CO gases and H2At least part of gas returns to the second gas stream.
It is produced during the Fischer-Tropsch reaction 9. according to any method of the preceding claims, further comprising utilizing Raw heat power generation, wherein the waste heat in power generation process is as described in the heat generated in the Fischer-Tropsch reaction Part is for regenerating the chemical absorbent.
10. a kind of integrated system, including：
CO2Absorption system has the entrance for first gas stream, and the first gas is flow to has CO gases and CO less2Gas Body, wherein the CO2Absorption system captures CO using chemical absorbent from the first gas stream2Gas is to generate and the first gas Body stream compares the CO of CO gases and low concentration with higher concentration2The second gas stream of gas；
Fischer-tropsch reactor, the fischer-tropsch reactor are connected to hydrogen (H2) source and it is connected to the CO2Absorption system is to receive State second gas stream, wherein the fischer-tropsch reactor be used for from the H2Gas and from described in the second gas stream The Fischer-Tropsch reaction catalysis of CO gases generates hydrocarbon；The wherein described Fischer-Tropsch reaction generates heat；
Heat exchanger, the heat that the heat exchanger is connected to the fischer-tropsch reactor to be generated during capturing the Fischer-Tropsch reaction Amount；And
CO2Desorption system, the CO2Desorption system is connected to the CO2Both absorption system and the heat exchanger, wherein by At least part of the heat of the heat exchanger capture of the fischer-tropsch reactor is connected in the CO2Desorption system Chemical absorbent described in hot recycling is to discharge captured CO in system2Gas.
11. integrated system according to claim 10, wherein in terms of the total volume percent of the first gas stream, it is described First gas stream has the CO gases and CO of at least 20 percents by volume (volume %)2The combined amount of gas.
12. the integrated system according to any one of claim 10 to 11, wherein the first gas stream includes 5 volumes hundred Divide nitrogen, 15 volume % to 50 volume %CO gases, the 5 volume % to 35 volume %CO than (volume %) to 60 volume %2Gas Body and 1 volume % to 35 volume % hydrogen.
13. the integrated system according to any one of claim 10 to 12, wherein the CO gas of the first gas stream Body and the CO2Molar ratio (the molal quantity of CO gases of gas:CO2The molal quantity of gas) it is 0.5:1 to 10:1.
14. integrated system according to claim 13, wherein the CO gases of the first gas stream and the CO2Gas Molar ratio (the molal quantity of CO gases of body:CO2The molal quantity of gas) it is 0.5:1 to 2.5:1.
15. the integrated system according to any one of claim 10 to 14, wherein for being generated in the Fischer-Tropsch reaction The H of the hydrocarbon2The CO gases in gas and the second gas stream are with 1:1 to 3:H in the range of 12Gas with Molar ratio (the H of CO gases2The molal quantity of gas：The molal quantity of CO gases) reaction.
16. the integrated system according to any one of claim 10 to 15, wherein the fischer-tropsch reactor is arrived at 200 DEG C It is operated with Co catalysts at temperature within the scope of 260 DEG C and the pressure in 1000kPa to 5000kPa ranges.
17. the integrated system according to any one of claim 10 to 16, wherein the Fischer-Tropsch reaction generates C5To C20 Hydrocarbon.
18. the integrated system according to any one of claim 11 to 17, wherein the CO from the fischer-tropsch reactor2Gas Body is provided to the CO2The entrance of absorption system.
19. the integrated system according to any one of claim 11 to 18, wherein from described in the fischer-tropsch reactor CO gases and H2At least part of gas returns to the fischer-tropsch reactor.
20. the integrated system according to any one of claim 11 to 19, wherein by the heat of the fischer-tropsch reactor The heat of exchanger capture is initially used for generating electricity, wherein remaining waste heat is used in the CO after the power generation2Solution Chemical absorbent described in hot recycling in desorption system.
CN201680066090.1A 2015-11-17 2016-11-14 Reduce the CO in industrial process2The method and system of discharge Pending CN108290109A (en)

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